In this work, methacrylated gelatin (GelMA) based hydrogels were fabricated with carboxybetaine methacrylate (CBMA) to manipulate the properties of the gelatin-based hydrogels, since CBMA is a much smaller compound compared to gelatin. With the incorporation of CBMA, these hydrogels demonstrated better mechanical properties, a slower degradation rate, and a controlled drug release rate compared with the GelMA alone group. GelMA/CBMA hydrogels also showed good cell viability. As in the in vivo test, vascular endothelial growth factor (VEGF)-loaded GelMA/CBMA hydrogels displayed certain degrees of angiogenesis. These results indicate that GelMA/CBMA hydrogels are biocompatible, and the properties of GelMA/CBMA hydrogels can be easily tuned with the ratio of CBMA. These characteristics make the GelMA/CBMA hydrogel a promising material for drug delivery and tissue engineering.